Design of stable mixed-metal MIL-101(Cr/Fe) materials with enhanced catalytic activity for the Prins reaction

Cristina Vallés-García, Effrosyni Gkaniatsou, Andrea Santiago-Portillo, Mónica Giménez-Marqués, Mercedes Álvaro, Jean Marc Greneche, Nathalie Steunou, Clémence Sicard, Sergio Navalón, Christian Serre, Hermenegildo García

Résultats de recherche: Contribution à un journal/une revueArticleRevue par des pairs

Résumé

This work highlights the benefit of designing mixed-metal (Cr/Fe) MOFs for enhanced chemical stability and catalytic activity. A robust and stable mixed-metal MIL-101(Cr/Fe) was prepared through a HF-free direct hydrothermal route with Fe3+ content up to 21 wt%. The incorporation of Fe3+ cations in the crystal structure was confirmed by 57Fe Mössbauer spectrometry. The catalytic performance of the mixed metal MIL-101(Cr/Fe) was evaluated in the Prins reaction. MIL-101(Cr/Fe) exhibited a higher catalytic activity compared to MIL-101(Cr), improved chemical stability compared to MIL-101(Fe) and a higher catalytic activity for bulky substrates compared to MIL-100(Fe). In situ infra-red spectroscopy study suggests that the incorporation of Fe3+ ions in MIL-101 structure leads to an increase in Lewis acid sites. It was thus concluded that the predominant role of Cr3+ ions was to maintain the crystal structure, while Fe3+ ions enhanced the catalytic activity.

langue originaleAnglais
Pages (de - à)17002-17011
Nombre de pages10
journalJournal of Materials Chemistry A
Volume8
Numéro de publication33
Les DOIs
Etat de la publicationPublié - 7 sept. 2020
Modification externeOui

Financement

Financial support by the Spanish Ministry of Economy and Competitiveness (Severo Ochoa, CTQ2018-890237-CO2-R1 and Maria de Maeztu, CEX2019-000919-M), is gratefully acknowledged. Generalidad Valenciana is also thanked for funding (Prometeo 2017/083). S. N. thanks nancial support by the Min-isterio de Ciencia, Innovación y Universidades (RTI 2018-099482-A-I00 project), Fundación Ramón Areces (XVIII Concurso Nacio-nal para la Adjudicación de Ayudas a la Investigación en Ciencias de la Vida y de la Materia, 2016), and Generalitat Valenciana grupos de investigación consolidables 2019 (ref: AICO/2019/214) project. E. G. thanks the ANR-11-LABEX-0039 (LabEx CHARM3AT) for nancial support. M. G.-M thanks support from “la Caixa” Foundation (LCF/BQ/PI19/11690022) and Generalitat Valenciana (SEJI/2020/036).

Bailleurs de fondsNuméro du bailleur de fonds
Fundación Ramón Areces
Generalitat ValencianaAICO/2019/214
Generalitat Valenciana
Investigación en Ciencias de la Vida y de la Materia
“la Caixa” FoundationSEJI/2020/036, LCF/BQ/PI19/11690022
“la Caixa” Foundation
Ministerio de Economía y Competitividad2017/083, CEX2019-000919-M, CTQ2018-890237-CO2-R1
Ministerio de Economía y Competitividad
Ministerio de Ciencia, Innovación y UniversidadesRTI 2018-099482-A-I00
Ministerio de Ciencia, Innovación y Universidades

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